Reuse of the solid residue from coal fly ash alumina extraction (FAAE) by acid leaching is problematic. Conversion of this solid residue into aluminum-rich zeolite (13X) and silicon-rich zeolite (ZSM-5) was investigated in this research. The FAAE residue was activated by alkali roasting with Na2CO3 powder (110% mass fraction) at 890 °C for 60 min. Silicon and aluminum were mainly present as two mineral phases, Na2SiO3 and NaAlSiO4, respectively, in the product obtained after roasting. The roasted product was dissolved in water (liquid/solid ratio of 2) after 20 min at 100 °C. The water-leaching liquor was investigated for total conversion to aluminosilicate zeolites without external aluminum or silicon addition. Hydrothermal synthesis of aluminum-rich zeolite 13X was successful after fine tuning of the conditions, although the filtrate had an unusually high SiO2/Al2O3 molar ratio. Production of 13X consumed a large amount of aluminum, which increased the Si/Al ratio to a level suitable for synthesis of ZSM-5. The synthesis of ZSM-5 from the mother liquor of 13X was proved feasible. The FAAE residue was transformed into high-value zeolite products by nearly 100%. Additionally, the tail liquid of this process, mainly containing Na2CO3, was completely recycled. This process could be used to realize high-efficiency and high-value utilization of similar aluminosilicate solid wastes.